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arXiv:2411.02389 · npj Computational Materials

Multidimensional coherent spectroscopy of correlated lattice systems

Jiyu Chen, Philipp Werner

Published May 9, 2025• 6 citations
arXivHTMLPDF

Abstract

Multidimensional coherent spectroscopy (MDCS) has been established in quantum chemistry as a powerful tool for studying the nonlinear response and nonequilibrium dynamics of molecular systems. More recently, the technique has also been applied to correlated electron materials, where the interplay of localized and itinerant states makes the interpretation of the spectra more challenging. Here we use the Keldysh contour representation of effective models and nonequilibrium dynamical mean field theory to systematically study the MDCS signals of prototypical correlated lattice systems. By analyzing the current induced by sequences of ultrashort laser pulses we demonstrate the usefulness of MDCS as a diagnostic tool for excitation pathways and coherent processes in correlated solids. We also show that this technique allows to extract detailed information on the nature and evolution of photo-excited nonequilibrium states.

DOI
10.1038/s41524-025-01619-0

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Abstract Multidimensional coherent optical spectroscopy (MDCS) is an elegant and versatile tool to measure the ultrafast nonlinear optical response of materials. Of particular interest for semiconductor nanostructures, MDCS enables the separation of homogeneous and inhomogeneous linewidths, reveals the nature of coupling between resonances, and is able to identify the signatures of many-body interactions. As an extension of transient four-wave mixing (FWM) experiments, MDCS can be implemented in various geometries, in which different strategies can be used to isolate the FWM signal and measure its phase. I review and compare different practical implementations of MDCS experiments adapted to the study of semiconductor materials. The power of MDCS is illustrated by discussing experimental results obtained on semiconductor nanostructures such as quantum dots, quantum wells, microcavities, and layered semiconductors.
Multi-dimensional coherent spectroscopy (MDCS) has become an extremely versatile and sensitive technique for elucidating the structure, composition, and dynamics of condensed matter, atomic, and molecular systems. The appeal of MDCS lies in its ability to resolve both individual-emitter and ensemble-averaged dynamics of optically created excitations in disordered systems. When applied to semiconductors, MDCS enables unambiguous separation of homogeneous and inhomogeneous contributions to the optical linewidth, pinpoints the nature of coupling between resonances, and reveals signatures of many-body interactions. In this review, we discuss the implementation of MDCS to measure the nonlinear optical response of excitonic transitions in semiconductor nanostructures. Capabilities of the technique are illustrated with recent experimental studies that advance our understanding of optical decoherence and dissipation, energy transfer, and many-body phenomena in quantum dots and quantum wells, semiconductor microcavities, layered semiconductors, and photovoltaic materials.
Abstract An introduction to multidimensional coherent spectroscopy (MDCS) is provided in this chapter. We start out by introducing MDCS in qualitative terms, as an extension of transient absorption spectroscopy. We proceed to discuss the meaning and utility of coherent spectroscopy more generally. We go on to discuss the specifics of MDCS as a specific form of coherent spectroscopy. Pulse sequences involved in generating MDCS plots are introduced. Finally, we discuss density matrix perturbation theory and double-sided Feynman diagrams, and the role of this formalism in simulating and interpreting MDCS.
This work covers two main results united by multidimensional coherent spectroscopy (MDCS): one experimental and one theoretical. MDCS is a nonlinear optical technique in which a sample is probed using a series of ultrashort pulses. Measurements are made while varying the relative time delays between the pulses, and the resulting spectra yield a much richer set of information compared to traditional linear spectroscopies. The experimental work concerns the negatively charged silicon-vacancy (SiV) center in diamond. We use two-pulse correlation (TPC) spectroscopy and rephasing MDCS to probe a diamond sample with a high density of implanted SiV centers. These spectra reveal a large number of spectral peaks, which can be grouped into two families of SiV centers using the MDCS spectra. By comparing spectra from two polarizations of the incident light, we associate the two families with two orientation groups within the diamond. We link the differences in the frequencies of the spectral peaks to strain intrinsic to our sample, and use the peak locations from both families to solve for the full strain tensor local to the laser spot. By measuring TPC spectra at multiple points on the sample, we track changes in the measured strain. We observe non-zero strain on the order or 1e-5 at every measured location, and observe variation in both the normal and shear strain in the sample. We interpret the strain as likely to be due to the high implantation density of silicon in the diamond. These results could be useful when using SiV centers as a strain gauge. The theoretical work uses simulations to calculate spectra. The simulations developed here begin by recursively generating a list of Feynman diagrams for a given signal pathway and system. The contributions due to each Feynman diagram are calculated and combined to find the complete spectrum. The code is designed to be very flexible, and can be used to simulate arbitrary types of MDCS spectra and energy level diagrams. We then apply the simulations to investigate the effects of correlated dephasing due to scattering events in the Markovian limit on MDCS of interacting systems. We derive a mathematical expression to represent the dephasing rate of a coherence in terms of the dephasing rates of the coherences from the constituent energy transitions and the correlation matrix of these transitions. This expression is applied to simulate double-quantum and higher-order n-quantum spectra of multiple interacting systems. For double-quantum spectra, correlated dephasing results in a higher double-quantum dephasing rate, and anticorrelated dephasing results in a lower double-quantum dephasing rate. Similar results are found for the n-quantum dephasing rate. Generally, for certain configurations, the many-body dephasing rate can be arbitrarily low, and the n-quantum linewidth can be arbitrarily narrow, although this requires some form of anticorrelation. These results could be useful in creating quantum sensors with higher sensitivities, since one limit of the sensitivity is the decoherence time of the system.
Double-quantum two-dimensional (2D) coherent spectroscopy (MDCS) is a powerful optical method that is used to study the optical properties of atomic and complex molecular systems and semiconductor materials. Double-quantum 2D spectra and particularly the peak line shapes on the spectra can also provide information about many-body interactions. We model 2D spectra by solving the optical Bloch equations and show the effects of correlation between coupled resonances, which also explains the discrepancies between the experimental results reported by multiple groups.